Functionalized Donor– π –Acceptor (D– π –A) Organic Linkers for Metal–Organic Frameworks with Extended Visible‐Light Absorption

Metal–organic frameworks (MOFs) are promising materials for photocatalytic hydrogen production. However, their efficiency is often limited by the optical properties of conventional organic linkers, such as terephthalic acid (TA). In this work, the synthesis of two novel triphenylamine‐based organic dyes (L0‐TA and L1‐TA) featuring a donor– π –acceptor (D –π –A) structure is reported. These dyes are functionalized with a terminal moiety analogous to aminoterephthalic acid, which serves as visible‐light‐absorbing linkers. These dyes retain the coordination ability required for MOF assembly while enhancing light‐harvesting properties. Crystallographic simulations confirm the structural compatibility of these colinkers in hybrid MOFs, providing a viable strategy to maintain MOF crystallinity while improving photocatalytic performance.